Performance evaluation of novel Ca/Mn-doped perovskite as a multifunctional material in chemical looping reverse water gas shift process for low-carbon fuels

The chemical looping reverse water gas shift (CL-RWGS) catalytic process offers a promising approach for decarbonizing energy-intensive industries. The CL-RWGS promotes the formation of surface oxygen vacancies in the material, which are subsequently replenished by extracting oxygen from CO 2 , resulting in syngas production. However, there remains a significant gap in the development of materials that not only exhibit redox activity but also enable in-situ carbonation, offering dual functionality for enhanced CO 2 utilization. This study introduces a novel calcium- and manganese-doped LaNiO 3 perovskite, designed for integrated CO 2 sorption and in-situ utilization during CL–RWGS process. Comprehensive characterization confirmed the material’s crystalline structure, porosity, and successful incorporation of Ca and Mn dopants. Thermogravimetric analysis (TGA) across 700 – 900 °C revealed a peak oxygen storage capacity of 1.97 mmol O 2 /g and demonstrated excellent redox stability, with less than 1% performance loss over 17 cycles. RWGS experiments conducted in a packed bed reactor demonstrated up to 57% CO 2 to CO conversion at 900 °C, approaching the thermodynamic equilibrium value of 60% under the same operating conditions. Moreover, an H 2 /CO molar ratio of ~2.0, suitable for Fischer-Tropsch synthesis, was achieved at 600 °C and 1.0 bar with a feed H 2 /CO 2 molar ratio of 1.0, attributed to CO 2 chemisorption via a carbonation-driven mechanism facilitated by the presence of CaO phase. These results suggest that the calcium- and manganese-doped LaNiO 3 perovskite is a highly promising multi-functional material for chemical looping-based CO 2 utilization technologies. • Ca/Mn co-doped LaNiO 3 was synthesized for CL-RWGS process. • Oxygen transfer capacity of 1.97 mmolO 2 /g was achieved with doped material. • 57% of CO 2 to CO conversion was obtained at 900 °C in RWGS stage. • CL-RWGS at 600 °C yielded syngas with a molar ratio of 2.0 suitable for FTS. • CO 2 sorption was confirmed via carbonation-calcination cycles testing.